Spatially Resolved Light-Induced Ferroelectric Polarization in α-In2Se3/Te Heterojunctions.

Light-induced ferroelectric polarization in 2D layered ferroelectric materials holds promise in photodetectors with multilevel current and reconfigurable capabilities. However, translating this potential into practical applications for high-density optoelectronic information storage remains challenging. In this work, an α-In2Se3/Te heterojunction design that demonstrates spatially resolved, multilevel, nonvolatile photoresponsivity is presented. Using photocurrent mapping, the spatially localized light-induced poling state (LIPS) is visualized in the junction region. This localized ferroelectric polarization induced by illumination enables the heterojunction to exhibit enhanced photoresponsivity. Unlike previous reports that observe multilevel polarization enhancement in electrical resistance, the device shows nonvolatile photoresponsivity enhancement under illumination. After polarization saturation, the photocurrent increases up to 1000 times, from 10-12 to 10-9 A under the irradiation of a 520 nm laser with a power of 1.69 nW, compared to the initial state in a self-driven mode. The photodetector exhibits high detectivity of 4.6×1010 Jones, with a rise time of 27 µs and a fall time of 28 µs. Furthermore, the device's localized poling characteristics and multilevel photoresponse enable spatially multiplexed optical information storage. These results advance the understanding of LIPS in 2D ferroelectric materials, paving the way for optoelectronic information storage technologies.

Emergent Ferroelectric Nematic and Heliconical Ferroelectric Nematic States in an Achiral "Straight" Polar Rod Mesogen.

Ferroelectric nematic liquid crystals (NFLCs) are distinguished by their remarkable polarization characteristics and diverse physical phenomena, sparking significant interest and excitement within the scientific community. To date, over 150 NFLC molecules are developed; however, there are no reports regarding straight linear polar molecules with a parallel alignment of the permanent dipole moment and the molecular axis. The straight polar mesogen nBOE exhibits an enantiotropic NF phase with a wide temperature window (up to 100 K) despite having a longer alkyl chain (up to n = 6) than the critical alkyl chain length of conventional models. Interestingly, nBOE with a medium-length alkyl chain displays an exotic phase sequence of NF-HCNF-SmXF during the elimination of positional displacement among adjacent molecules. Furthermore, the reflective color modulation of the HCNFLC over the entire VIS-NIR spectral regime by ultralow E-field (up to 0.14 V µm-1) is demonstrated.

Reconfigurable aJ-Level Ferroelectric Transistor-Based Boolean Logic for Logic-in-Memory.

Logic-in-memory (LIM) architecture holds great potential to break the von Neumann bottleneck. Despite the extensive research on novel devices, challenges persist in developing suitable engineering building blocks for such designs. Herein, we propose a reconfigurable strategy for efficient implementation of Boolean logics based on a hafnium oxide-based ferroelectric field effect transistor (HfO2-based FeFET). The logic results are stored within the device itself (in situ) during the computation process, featuring the key characteristics of LIM. The fast switching speed and low power consumption of a HfO2-based FeFET enable the execution of Boolean logics with an ultralow energy of lower than 8 attojoule (aJ). This represents a significant milestone in achieving aJ-level computing energy consumption. Furthermore, the system demonstrates exceptional reliability with computing endurance exceeding 108 cycles and retention properties exceeding 1000 s. These results highlight the remarkable potential of a FeFET for the realization of high performance beyond the von Neumann LIM computing architectures.

Antiferroelectric Heterostructures Memristors with Unique Resistive Switching Mechanisms and Properties.

A novel antiferroelectric material, PbSnO3 (PSO), was introduced into a resistive random access memory (RRAM) to reveal its resistive switching (RS) properties. It exhibits outstanding electrical performance with a large memory window (>104), narrow switching voltage distribution (±2 V), and low power consumption. Using high-resolution transmission electron microscopy, we observed the antiferroelectric properties and remanent polarization of the PSO thin films. The in-plane shear strains in the monoclinic PSO layer are attributed to oxygen octahedral tilts, resulting in misfit dislocations and grain boundaries at the PSO/SRO interface. Furthermore, the incoherent grain boundaries between the orthorhombic and monoclinic phases are assumed to be the primary paths of Ag+ filaments. Therefore, the RS behavior is primarily dominated by antiferroelectric polarization and defect mechanisms for the PSO structures. The RS behavior of antiferroelectric heterostructures controlled by switching spontaneous polarization and strain, defects, and surface chemistry reactions can facilitate the development of new antiferroelectric device systems.

Reversible oxidation of ethylene on ferroelectric BaTiO3(001): An X-ray photoelectron spectroscopy study.

Adsorption and desorption of ethylene on BaO-terminated (001) barium titanate are investigated by X-ray photoelectron spectroscopy. Carbon is found in an oxidized state, at a binding energy similar to that resulting from CO adsorption on BaTiO3(001). The amount of carbon adsorbed on the surface is also similar to the case of CO/BaTiO3(001). Upon heating the substrate up to the loss of its ferroelectric polarization, the C 1s signal from the oxidized spectral region vanishes. At the same time, there was no noticeable oxygen depletion of the surface after repeated C2H4 adsorption and desorption. The substrate remains stable after repeated oxidative adsorption and desorption of ethylene. Desorption occurs at different temperatures, depending on the adsorption temperature, which suggests different adsorption geometries: non-dissociated adsorption at high temperature with ethylene bond on two surface oxygen atoms, and locally dissociated adsorption at lower temperatures, in "formaldehyde-like" local configurations.

Magnetic-anisotropy modulation in multiferroic heterostructures by ferroelectric domains from first principles.

First-principles calculations incorporating spin-orbit coupling are presented for a multiferroic material as a ferromagnetic/ferroelectric junction. We simulate the interface effect that cannot be described by the single-phase bulk. The in-plane uniaxial magnetic-anisotropy of Co2FeSi is observed when the ferroelectric domain is polarized parallel to the interface, whereas the magnetic anisotropy is significantly different in the plane for the electrical polarization perpendicular to the interface. While the single-phase effect dominates the main part of the modulation of the magnetic anisotropy, symmetry breaking due to the interfacial effect is observed in the ferromagnetic ultrathin films. The origin of the modulated magnetic-anisotropy can be attributed to the shifting of specific energy bands in Co2FeSi when the ferroelectric domain is modified.

The origin of strain-induced magnetocrystalline anisotropy in multiferroic Co₂FeSi/BaTiO₃(001) heterostructures is clarified by first-principles electron theory. The magnetic anisotropy is modified by interface effects for ultrathin Co₂FeSi films.

Distinguishing the Rhombohedral Phase from Orthorhombic Phases in Epitaxial Doped HfO2 Ferroelectric Films.

Epitaxial strain plays an important role in the stabilization of ferroelectricity in doped hafnia thin films, which are emerging candidates for Si-compatible nanoscale devices. Here, we report on epitaxial ferroelectric thin films of doped HfO2 deposited on La0.7Sr0.3MnO3-buffered SrTiO3 substrates, La0.7Sr0.3MnO3 SrTiO3-buffered Si (100) wafers, and trigonal Al2O3 substrates. The investigated films appear to consist of four domains in a rhombohedral phase for films deposited on La0.7Sr0.3MnO3-buffered SrTiO3 substrates and two domains for those deposited on sapphire. These findings are supported by extensive transmission electron microscopy characterization of the investigated films. The doped hafnia films show ferroelectric behavior with a remanent polarization up to 25 µC/cm2 and they do not require wake-up cycling to reach the polarization, unlike the reported polycrystalline orthorhombic ferroelectric hafnia films.

Flexoelectric Enhancement of Strain Gradient Elasticity Across a Ferroelectric-to-Paraelectric Phase Transition.

We study the temperature dependent elastic properties of Ba0.8Sr0.2TiO3 freestanding membranes across the ferroelectric-to-paraelectric phase transition using an atomic force microscope. The bending rigidity of thin membranes can be stiffer compared to stretching due to strain gradient elasticity (SGE). We measure the Young's modulus of freestanding Ba0.8Sr0.2TiO3 drumheads in bending and stretching dominated deformation regimes on a variable temperature platform, finding a peak in the difference between the two Young's moduli obtained at the phase transition. This demonstrates a dependence of SGE on the dielectric properties of a material and alludes to a flexoelectric origin of an effective SGE.

Ferroelectric Modulation of Quantum Emitters in Monolayer WS2.

Quantum photonics promises significant advances in secure communications, metrology, sensing, and information processing/computation. Single-photon sources are fundamental to this endeavor. However, the lack of high-quality single photon sources remains a significant obstacle. We present here a paradigm for the control of single photon emitters (SPEs) and single photon purity by integrating monolayer WS2 with the organic ferroelectric polymer poly(vinylidene fluoride-co-trifluoroethylene) (P(VDF-TrFE)). We demonstrate that the ferroelectric domains in the P(VDF-TrFE) film control the purity of single photon emission from the adjacent WS2. By switching the ferroelectric polarization, we reversibly tune the single photon purity between the semiclassical and quantum light regimes, with single photon purities as high as 94%. This demonstrates a method for modulating and encoding quantum photonic information, complementing more complex approaches. This multidimensional heterostructure introduces an approach for control of quantum emitters by combining the nonvolatile ferroic properties of a ferroelectric with the radiative properties of the zero-dimensional atomic-scale emitters embedded in the two-dimensional WS2 semiconductor monolayer.

Light-Adapted Optoelectronic-Memristive Device for the Artificial Visual System.

With the development of artificial intelligence systems, it is necessary to develop optoelectronic devices with photoresponse and storage capacity to simulate human visual perception systems. The key to an artificial visual perception system is to integrate components with both sensing and storage capabilities of illumination information. Although module integration components have made useful progress, they still face challenges such as multispectral response and high energy consumption. Here, we developed a light-adapted optoelectronic-memristive device integrated by an organic photodetector and ferroelectric-based memristor to simulate human visual perception. ITO/P3HT:PC71BM/Au as the light sensor unit shows a high on/off ratio (Iph/Id) reaching ∼5 × 104 at 0 V. The memristor unit, consisting of ITO/CBI@P(VDF-TrFE)/Cu, has a RON/ROFF ratio window of ∼106 under 0.05 V read voltage and ultralow power consumption of ∼1 pW. Moreover, the artificial visual perception unit shows stable light-adapted memory windows under different wavelengths of irradiation light (400, 500, and 600 nm; they meet the spectral range of human visual recognition) and can clearly identify the target image ("T" shape) because of the apparent contrast, which results from the high ROFF/RON ratio values. These results provide a potential design strategy for the development of intelligent artificial vision systems.

Evolution of Ferroelectricity in Sr0.6Ba0.4Nb2O6-BaTiO3 Solid Solution with a Strong Electrocaloric Effect.

In conventional knowledge, ferroelectric solid solutions were formed between members belonging to the same crystal structure family. Since both tungsten bronze and perovskite structures are constructed by connecting the corner-sharing oxygen octahedra, it offers a possibility for formatting an unusual solid solution between these two families. Herein, (1 - x)Sr0.6Ba0.4Nb2O6-xBaTiO3, (1 - x)SBN-xBT, solid solutions were synthesized and the solution mechanism was resolved from a structure viewpoint. With increasing BT content, the solid solution persists of tetragonal tungsten bronze structure, but the lattice parameter a (= b) decreases whereas c increases, resulting in the significant reduction of grains anisotropy. The ferroelectric-relaxor phase transition temperature shows a monotonic increase as x increases. However, the ferroelectricity evolution is not monotonous as a function of BT content because of the competitive effects of Ba and Ti on the property. As a result, the x = 0.10 ceramic shows the strongest ferroelectricity and a remarkable electrocaloric effect of 1.4 K near room temperature. This work challenges the traditional view of solid solution formation and provides an alternative way to modulate the structure and properties of ferroelectrics.

Ultralow Energy Consumption and Fast Neuromorphic Computing Based on La0.1Bi0.9FeO3 Ferroelectric Tunnel Junctions.

Low-power and fast artificial neural network devices represent the direction in developing analogue neural networks. Here, an ultralow power consumption (0.8 fJ) and rapid (100 ns) La0.1Bi0.9FeO3/La0.7Sr0.3MnO3 ferroelectric tunnel junction artificial synapse has been developed to emulate the biological neural networks. The visual memory and forgetting functionalities have been emulated based on long-term potentiation and depression with good linearity. Moreover, with a single device, logical operations of "AND" and "OR" are implemented, and an artificial neural network was constructed with a recognition accuracy of 96%. Especially for noisy data sets, the recognition speed is faster after preprocessing by the device in the present work. This sets the stage for highly reliable and repeatable unsupervised learning.

Electronic and Transport Engineering of A-Type Antiferromagnets with Ferroelectric Sandwich Structure: Toward Multistate Nonvolatile Memory Applications.

Achieving higher-order multistates with mutual interstate switching at the nanoscale is essential for high-density storage devices; yet, it remains a significant challenge. Here, we demonstrate that integrating A-type antiferromagnetic semiconductors sandwiched between ferroelectric layers is an effective strategy to achieve high-performance multistate data storage. Taking the Sc2CO2/VSi2P4 bilayer (bi-VSi2P4)/Sc2CO2 van der Waals multiferroic heterostructure as an example, our first-principles calculations show that by switching the polarization direction of the upper and bottom ferroelectric Sc2CO2 layers, antiferromagnetic bi-VSi2P4 can exhibit four distinct states with different band structures. The intriguing band structure engineering stems from the polarization-field-induced band shift and interface charge transfer. Accordingly, the proposed Sc2CO2/bi-VSi2P4/Sc2CO2-based multiferroic device can achieve four different resistance states, accompanied by fully spin-polarized currents and giant tunneling electroresistance ratios. Our results propose a viable strategy for realizing nonvolatile electrical control of antiferromagnets at the nanoscale and provide insights into the development of advanced memories.

Nonvolatile Electric Control of Rashba Spin Splitting in Sb/In2Se3 Heterostructure.

Ferroelectric Rashba semiconductors (FRS) are highly demanded for their potential capability for nonvolatile electric control of electron spins. An ideal FRS is characterized by a combination of room temperature ferroelectricity and a strong Rashba effect, which has, however, been rarely reported. Herein, we designed a room-temperature FRS by vertically stacking a Sb monolayer on a room-temperature ferroelectric In2Se3 monolayer. Our first-principles calculations reveal that the Sb/In2Se3 heterostructure exhibits a clean Rashba splitting band near the Fermi level and a strong Rashba effect coupled to the ferroelectric order. Switching the electric polarization direction enhances the Rashba effect, and the flipping is feasible with a low energy barrier of 22 meV. This Rashba-ferroelectricity coupling effect is robust against changes of the heterostructure interfacial distance and external electric fields. Such a nonvolatile electrically tunable Rashba effect at room temperature enables potential applications in next-generation data storage and logic devices operated under small electrical currents.

Polarization-Switchable Electrochemistry of 2D Layered Bi2O2Se Bifunctional Microreactors by Ferroelectric Modulation.

Ferroelectric catalysts are known for altering surface catalytic activities by changing the direction of their electric polarizations. This study demonstrates polarization-switchable electrochemistry using layered bismuth oxyselenide (L-Bi2O2Se) bifunctional microreactors through ferroelectric modulation. A selective-area ionic liquid gating is developed with precise control over the spatial distribution of the dipole orientation of L-Bi2O2Se. On-chip microreactors with upward polarization favor the oxygen evolution reaction, whereas those with downward polarization prefer the hydrogen evolution reaction. The microscopic origin behind polarization-switchable electrochemistry primarily stems from enhanced surface adsorption and reduced energy barriers for reactions, as examined by nanoscale scanning electrochemical cell microscopy. Integrating a pair of L-Bi2O2Se microreactors consisting of upward or downward polarizations demonstrates overall water splitting in a full-cell configuration based on a bifunctional catalyst. The ability to modulate surface polarizations on a single catalyst via ferroelectric polarization switching offers a pathway for designing catalysts for water splitting.

Role of Annealing with Electric Field Toward Improvement of Ferroelectric and Electroactive Properties of PVDF Copolymer and Terpolymer Thin Films.

The present study elucidates the role of annealing with electric field on lamellar crystalline structure and molecular orientation of polymer chains in ferroelectric copolymer (P(VDF-TrFE)) and ferroelectric terpolymer (P(VDF-TrFE-CFE)) spin-coated thin films. The ferroelectric polymer thin films annealed under an electric field support the growth of nanostructure with an "edge-on" lamellar crystalline structure having in-plane molecular chain orientation. The poled P(VDF-TrFE) thin films have higher remnant polarization (Pr) ≈6.2 µC cm-2 and saturation polarization (Ps) ≈8.2 µC cm-2 at an applied electric field of 250 MV/m compared to unpoled thin films having Pr ≈4.7 and Ps ≈6.2 µC cm-2. Also, poled P(VDF-TrFE) thin films show lower coercive field (Ec) ≈94 MV/m compared to an unpoled thin film having Ec ≈105 MV/m. Similarly, poled PVDF-TrFE-CFE thin film shows better ferroelectric properties having Pr ≈0.4 and Ps ≈5.7 µC cm-2 at an applied electric field of 200 MV m-1 compared to unpoled thin films having Pr ≈0.4 and Ps ≈4.1 µC cm-2. The storage energy efficiency of unpoled and poled P(VDF-TrFE-CFE) thin films is measured to be ≈75% and 80%. Annealing of ferroelectric P(VDF-TrFE) polymer thin films under an electric field demonstrates improved ferroelectric and electroactive properties.

Electric Field-Manipulated Optical Chirality in Ferroelectric Vortex Domains.

Manipulating optical chirality via electric fields has garnered considerable attention in the realm of both fundamental physics and practical applications. Chiral ferroelectrics, characterized by their inherent optical chirality and switchable spontaneous polarization, are emerging as a promising platform for electronic-photonic integrated circuits applications. Unlike organics with chiral carbon centers, integrating chirality into technologically mature inorganic ferroelectrics has posed a long-standing challenge. Here, the successful introduction of chirality is reported into self-assembly La-doped BiFeO3 nanoislands, which exhibit ferroelectric vortex domains. By employing synergistic experimental techniques with piezoresponse force microscopy and nonlinear optical second-harmonic generation probes, a clear correlation between chirality and polarization configuration within these ferroelectric nanoislands is established. Furthermore, the deterministic control of ferroelectric vortex domains and chirality is demonstrated by applying electric fields, enabling reversible and nonvolatile generation and elimination of optically chiral signals. These findings significantly expand the repertoire of field-controllable chiral systems and lay the groundwork for the development of innovative ferroelectric optoelectronic devices.

Enhancing Thermoelectric and Cooling Performance of Bi0.5Sb1.5Te3 through Ferroelectric Polarization in Flexible Ag/PZT/PVDF/Bi0.5Sb1.5Te3 Film.

Bi2Te3-based thin films are gaining recognition for their remarkable room temperature thermoelectric performance. Beyond the conventional "process-composition-performance" paradigm, it is highly desirable to explore new methods to enhance their performance further. Here, we designed a sandwich-structured Ag/PZT/PVDF/Bi0.5Sb1.5Te3(BST) thin film device and effectively regulated the performance of the BST film by controlling the polarization state of the PZT/PVDF layers. Results indicate that polarization induces interlayer charge redistribution and charge transfer between PZT/PVDF and BST, thereby achieving the continuous modulation of the electrical transport characteristics of BST films. Finally, following polarization at a saturation voltage of 3 kV, the power factor of the BST film increased by 13% compared to the unpolarized condition, reaching 20.8 µW cm-1 K-2. Furthermore, a device with 7 pairs of P-N legs was fabricated, achieving a cooling temperature difference of 11.0 K and a net cooling temperature difference of 2.4 K at a current of 10 mA after the saturation polarization of the PZT/PVDF layer. This work reveals the critical effect of introducing ferroelectric layer polarization to achieve excellent thermoelectric performance of the BST film.

Ferroelectric Aluminum Scandium Nitride Transistors with Intrinsic Switching Characteristics and Artificial Synaptic Functions for Neuromorphic Computing.

Aluminum Scandium Nitride (Al1-xScxN) has received attention for its exceptional ferroelectric properties, whereas the fundamental mechanism determining its dynamic response and reliability remains elusive. In this work, an unreported nucleation-based polarization switching mechanism in Al0.7Sc0.3N (AlScN) is unveiled, driven by its intrinsic ferroelectricity rooted in the ionic displacement. Fast polarization switching, characterized by a remarkably low characteristic time of 0.00183 ps, is captured, and effectively simulated using a nucleation-limited switching (NLS) model, where the profound effect of defects on the nucleation and domain propagation is systematically studied. These findings are further integrated into Monte Carlo simulations to unravel the influence of the activation energy for ferroelectric switching on the distributions of switching thresholds. The long-term reliability of devices is also confirmed by time-dependent dielectric breakdown (TDDB) measurements, and the effect of thickness scaling is discussed. Ferroelectric field-effect transistors (FeFETs) are demonstrated through the integration of AlScN and 2D MoS2 channel, where biological synaptic functions can be emulated with optimized operation voltage. The artificial neural network built from AlScN-based FeFETs achieves 93.8% recognition accuracy of handwritten digits, demonstrating the potential of ferroelectric AlScN in future neuromorphic computing applications.

Ferroelectrovalley in Two-Dimensional Multiferroic Lattices.

Engineering the valley index is essential and highly sought for valley physics, but currently, it is exclusively based on the paradigm of the challenging ferrovalley with spin-orientation reversal under a magnetic field. Here, an alternative strategy, i.e., the so-called ferroelectrovalley, is proposed to tackle the insurmountable spin-orientation reversal, which reverses the valley index with the feasible ferroelectricity. Using symmetry arguments and the tight-binding model, the C2z rotation is unveiled to be able to take the place of time reversal for operating the valley index in two-dimensional multiferroic kagome lattices, which enables a ferroelectricity-engineered valley index, thereby generating the concept of a ferroelectrovalley. Based on first-principles calculations, this concept is further demonstrated in the breathing kagome lattice of single-layer Ti3Br8, wherein ferroelectricity couples with the breathing process. These findings open a new direction for valleytronics and 2D materials research.